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Coupling photocatalytic CO2 reduction and CH3OH oxidation for selective dimethoxymethane production.

Yixuan Wang | Yang Liu | Lingling Wang | Silambarasan Perumal | Hongdan Wang | Hyun Ko | Chung-Li Dong | Panpan Zhang | Shuaijun Wang | Ta Thi Thuy Nga | Young Dok Kim | Yujing Ji | Shufang Zhao | Ji-Hee Kim | Dong-Yub Yee | Yosep Hwang | Jinqiang Zhang | Min Gyu Kim | Hyoyoung Lee
Nature communications | 2024

Currently, conventional dimethoxymethane synthesis methods are environmentally unfriendly. Here, we report a photo-redox catalysis system to generate dimethoxymethane using a silver and tungsten co-modified blue titanium dioxide catalyst (Ag.W-BTO) by coupling CO2 reduction and CH3OH oxidation under mild conditions. The Ag.W-BTO structure and its electron and hole transfer are comprehensively investigated by combining advanced characterizations and theoretical studies. Strikingly, Ag.W-BTO achieve a record photocatalytic activity of 5702.49 µmol g-1 with 92.08% dimethoxymethane selectivity in 9 h of ultraviolet-visible irradiation without sacrificial agents. Systematic isotope labeling experiments, in-situ diffuse reflectance infrared Fourier-transform analysis, and theoretical calculations reveal that the Ag and W species respectively catalyze CO2 conversion to *CH2O and CH3OH oxidation to *CH3O. Subsequently, an asymmetric carbon-oxygen coupling process between these two crucial intermediates produces dimethoxymethane. This work presents a CO2 photocatalytic reduction system for multi-carbon production to meet the objectives of sustainable economic development and carbon neutrality.

Pubmed ID: 39025876

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Associated grants

  • Agency: National Research Foundation of Korea (NRF),
    Id: NRF-2022R1A2C2093415
  • Agency: Korea Basic Science Institute (KBSI),
    Id: 2022R1A6C101A751
  • Agency: China Scholarship Council (CSC),
    Id: 202208260012

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